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AAKlementiov Estimation of the Pu-239 Releases to the Atmosphere from the Hanford Site. December 21, 1995,
Repoit to Tom H, Foulds, Hanford Litigation Office, Seattle. om

Table 3

Major stages in development of the emission control equipment

GRR-0.0024

control development are presented in the 3rd row in Table 3. Clearly, overall
particulate decontamination factor (when beth ventilation lines are considered) dhiring
month & is equal to

ODE H)% = (0.72: DF(k) + 0.28-DF°(k) )100% .

Values of ODF() pertaining to each particular period of the emission control
development are presented in the 4th row in Table 3.

5. ESTIMATION OF THE OVERALL RELEASE FACTOR

Two figures nmst be known to estimate the amounts of Pu-239 released during a
month k: monthly averaged release factor ORF(&) and Pi?) - amount of Pu-239
processed during the month. The latter figures are available from historical records.



AAKlamentioy Estimation of the Pi:-239 Releases to the Atmosphere from the Hanford Site. December 21, 1995.
Report to Tom H. Foulds, Hanford Litigation Office, Seattle.

INTRODUCTION

HEDR estimates of the amounts of Pu-239 released to the atmosphere were reported in
[He94]. Four separations plants stacks were considered in [He94] as the sources of the
releases. Since then, new operational data compiled from the historical records pertaining
to the Pu-239 releases from the Hanford Site became available. The data are presented in
this report in Appendix A, Table Al. The new operational data were used in this report for
reestimation of the Pu-239 releases accounting for more than the four sources considered in
[He94]. Following groups of the Pu-239 emitters were analyzed in this report:

© Separations plant stacks;

© 100 areas reactor stacks;

¢ 224 concentration building roof fans;
© Z-plant stack.

1. DEFINITIONS

The concept of Pu-239 release factor calculation is presented on Figure 1. Amount of

Pu-239 dissolved during a given unit of time is suggested to be equal to PU;. Part of

it, PU> , will leave the solution, will enter the ventilation systems, and eventually it
[a

ea

PUs

Figure 1
Concept of release factor calculation



AAKlementiev Estimauon of the Pu-239 Releases to the Atmosphere from the Hanford Site, December 21, 1995.
‘Repertto Tom H. Foukds, Hanford Litigation Office, Seattle,

stage, additional 2.8 millicurie was released from 224 concentration building roof fans. the
T-Plant stack during the separation process, Clearly, the amount of Pu-239 released from
the roof fans of the 224 building was about 11 times higher than what was released from
the T-Plant stack. One can see from three examples presented in Table 8 that the releases

from the 224 building roof fans always exceeded the releases from the corresponding
separation plant stacks.

Table 8
Releases from 224 concentration building roof fans

Reference Stack location Period | Period | Pu-239 [| Pu239 | Pu-239 | Pu-239 | Ratio:
begin | end | released: | released: | processed: | released: | Alternative
Alternative {Alternative} Ci/Mo | HEDR | to HED!
Cilday Cifmo Cifmo
‘HW-24664} CONCENT. BLDG CELL] 5/1/52] 5/31/52] 2.106E-05|
VENT B 224-1}
HW-24664} CONCENT. BLDG CELL 5/1/52} 5/31/52) 3.862E-05}
VENT C 224-T]
HW-24664| CONCENT. BLDG CELL| 5/1/52] 5/31/52] 3.070E-05| 2.80B-03 650} 2.60E-04| YW
VENT D 224-T|
HW-25531] CONCENT. BLDG CELL] 8/1/52] 8/31/52] 2.198E-05}
VENT B 224-7]
‘HW-25531] CONCENT. BLDG CELL] 8/1/52 8/31/52] 3.684E-06|
VENT C 224-1]
HW-25531] CONCENT. BLDG CELL 8/1/52] 8/31/52] 2239804! 7.70503 1050} 4.19E-04) 18
~__ VENT D 224-T|
HW-27938] CONCENT. BLDG CELL! 4/1/53] 4/30/53, 6.754506]

HW-27938| CONCENT. BLDG CELL] 4/1/53[ 4/30/53) 4.912-06|

HW-27938| CONCENT. BLDG CELL 4/1/53] 40/53] 6.754B-06| 5.53E-04 427) L-TIE-04 3

9, Z-PLANT

The plutonium recovery and finishing operation facility, or Z Plant, began operation in late
1949 to process plutonium and to prepare plutonium products. Plutonium was brought to
Z Plant as the liquid nitrate solution, then processed forming the metal. Z-Plant had
individual vent system and stack as it is indicated in [Ja72].

Let us define release factor for Z Plant (RF-Z) as the ratio

RF-Z = Amount of Pu-239 released from Z Plant / Amount of Pu-239 processed in Z Plant.

The values of RF-Z based on the data from the source spreadsheet and on the assumption
that all Pu-239 from the separation plants was brought to Z Plant, are presented in Table 9.

10



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: 19 ‘On DBeg



2.0 Background and Qualifications

I am a professional engineer with over 12 years of experience in the power production and
environmental field. My doctoral research involved computational fluid dynamics (CFD), with
focus on environmental flows.

My understanding of the environmental field comes, among other experiences, from being the:

Q Main author of ISC View, one of the three leading air dispersion models used in the U.S.A.
and abroad.

. Q Main author of BPIP View, the most advanced commercial Building Profile Input Program,
3 to predict the effect of building downwash on elevated point sources.

GQ Main author of Screen View, a screening air dispersion model adopted by major U.S.A. and
Canadian universities within various their air dispersion modelling courses.

9 Main Author of SLAB View, a dense gas dispersion model, used for emergency release
analysis and predictions.

Q Main Author of IRAP View, a health and ecological risk assessment package from toxic air
emissions. The U.S. EPA as their main chronic health risk assessment package in this area
has adopted this package.

a Author of “Air Dispersion Modelling ~ A Visual Approach”, a book to be published by
December 1999. This book deals with air dispersion models for short term, Gaussian plume,
dense gas releases, Gaussian puff models for long-range transport, and risk assessment using
a multi-pathway approach.

a Co-author of Visual MODFLOW, a three-dimensional groundwater flow and transport code
which sold more than 1,000 copies.

a Co-authors of Flowpath 5.0, a two-dimensional groundwater flow and water table drawdown
analyses package, which sold more than 1,000 copies.

Q Co-author of Airflow Soil Vapour Extraction, a package to compute the extraction of volatile
organic compounds from the vadose zone of contaminated soils. _.

Note that ISC View, BPIP View, and Screen View were published in book format and have their
own ISBN numbers.

My experience on air dispersion modelling include more then 60 different works, such as:

a Risk assessment support work and review for the new U.S. EPA risk assessment protocol,
“Screening Level Human Health Risk Assessment at Hazardous Waste Combustion
Facilities”.

a Transit pollution in the City of Toronto and the City of Vaughan.

Dense gas dispersion in oil refineries.

a Regulatory models for various industries, particulate emissions from quarries and cement
plants.

Q Pollution impacts from coal fired power plants and coke manufacturing units.

a Extemal consultant to various engineering consulting companies on topics related to air
dispersion modelling, such as meteorological data, emergency dense gas releases, regulatory
modelling, odors, particulates, and VOCs.

Qa



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AA Kiementiev Estimation of the Pu-239 Releases to the Aomosphere from the Hanford Size. December 21, 1995:
‘Report to Tom HI. Foulds, Hanford Litigation Office, Seattle.

The values RF(&) are unknown, but they can be found from the overall decontamination
efficiency figures in the following way.

Let two figures be known for a month £*: the overall release factor ORF(k*) and overall
decontamination factor ODF(k*)%. With the use of (3) we can estimate generic release
ratio as:

(——GRR(K*) = (ORFYK*) / (100% - ODF(k*) })-100%.

Note that ORF(k*) is known for some given month x only, and it is still unknown for the
arbitrary month &.

For example, after the silver reactor and fiberglass filter were installed in B and T Plants
instead of the water scrubbers, the overall particulate decontamination factor became equal
to 99.76% [BI93]. On the other hand, overall release factor pertaining to B and T Plants
Operations in the first four months of 1952 is reported in [He94] as equal to 4-107,
Therefore,

GRR = 4-107 / (100% - 99.76%)-100% = 1.7-107.
It should be noted that 4-10” is not the only estimate of the overall release factor available

from the historical records. Three different estimates of GRR based on different overall
release factor measurements are given in Table 4. ©

Table 4

Estimates of generic release ratio based on different overall release factor measurements

GRR reference [ B & T Plants, 1-4/52 B Plant, 4/52 B Plant, 4/52, T Plant, 4/52, 4/55
[He94] [He94] and this report This report
Generic release ratio 4-107 6.7107 1.4-10°
GRR
Overall release factor 17-107 28-107 58-107
ORF

We now assume that the value of generic release ratio remains the same for all months of
production, and it is equal to GRR. Next step is to find the overall release factor ORF() for
an arbitrary month & It is, by definition, equal to

(9) ORF(K) = GRR (100% - ODF(K)9)/100% ,

where ODF) can be found from the last row in Table 5.



1.0 Introduction

Tom Foulds and Associated Counsel have retained me to compare the concentration predictions
by the HEDR codes against the vegetation concentration measurements. This study is part of the
investigation of the exposure of radioiodine resulting from nuclear fuel processing’ and ‘other
activities at the Hanford site, near Richland, WA.

A number of review activities were carried out from June 17 to June 30, 1997 and from Jan 12 to
Mar 26, 1998. This report will discuss only activities during those time period relevant to
determine the radiation measurements, based ‘on sagebrush leaves samples, of iodine-131 from
the Hanford emissions.

The reconstruction of the source-term executed by the Pacific Northwest Laboratories requires a
reassembly and considerable restoration. The set of computer codes developed, known as the
Hanford Environmental Reconstruction (HEDR) codes, are composed of separate codes for
various related simulations. The documentation, computer codes, and data are loosely dispersed
over paper records, file formats, and computer platforms. Measurement tables are reported
without proper units and sample geographical location is difficult to determine. Most sample
locations are indicated by cell numbers, others by node numbers, and some by road number.
Errors and revisions are not readily and concisely available, which causes confusion and delays
in the analysis of the procedures.

Therefore, this report represents my best effort to achieve its objectives:

Namely to take the output of the HEDR model known as DESCARTES, which calculates
‘vegetation concentrations and compares these predictions with the historical vegetation records
as given in PNWD-2177 and PNWD-2145 over the same years, 1945 through 1951.



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* Additionally, I develop research work with the Canadian National Research Counsel. I am also
a trainer in intemational courses in topics related to air dispersion modelling, risk assessment,
and environmental management systems.



ESTIMATION OF PU-239 RELEASES TO THE
ATMOSPHERE FROM THE HANFORD SITE

Prepared for: Tom H. Foulds, Hanford Litigation Office, Seattle
Prepared by: A. A. Klementiev, Consultant

December 21, 1995

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AAKlementiov Estimation of the Pu-239 Relaases to the Atmosphere from the Hanford Site. Decestber 21, 1995,
Report to Tom H. Foulds, Hanford Litigation Office, Seattle,

TABLE OF CONTENTS

INTRODUCTION

1, DEFINITIONS

2. METHOD OF THE Pu-239 RELEASES ESTIMATION: HEDR APPROACH
3. BLASEWITZ’ CRITICISM

4, CHRONOLOGY

5. ESTIMATION OF THE OVERALL RELEASE FACTOR

6. ESTIMATION OF THE RELEASES FROM THE SEPARATIONS PLANT
STACKS

7. 100 AREAS REACTOR STACKS
8. 224 CONCENTRATION BUILDING ROOF FANS
9. Z-PLANT

10. FINDINGS

" REFERENCES

APPENDIX A.

APPENDIX B

10

1

13

14

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Hanford Litigation - HEDR Vegetation Radiation Model Comparison

Prepared for
Tom H. Foulds and Associated Counsel
for the ,
Hanford Radiation Litigation

by

Prof. Jesse L. Thé, PhD., P-Eng.

Lakes Environmental Consultants Inc.

February 26, 1999



Table of Contents

1.0 Introduction. .......00 dtanesearonses
2.0 Background and Qualifications
3.0 Overviéw of RATCHET........ woeeneraeees
Figure 3.1 — Terrain Elevation over’ modeled domain
Figure 3.2 ~ UTM Coordinates of modeled domain

4.0 RATCHET Validation Reports
4.1 Validation Procedure ...
4.2 Air Dispersion Model...
4.3 Terrain Elevations...
4.4 Local Meteorology ..
4.5 Wet-to-dry Weight Conversions
4.6 Equipment Calibration ..............
4.7 Gamma Ray Spectroscopy Correction.
4.8 Recommendations for the Hanford Air Dispersion Model Validation
5.0 Data Processing and Analysis of Results
5.1 Data availability
5.2 Data Pre-processing
5.3 Data Processing
§.3.1 Initial Tests
Figure 5.1 ~ Large range, small segmentation (observed — modeled)
Figure 5.2 ~ Large range, small segmentation (observed"4.8 ~ modeled)
Figure 5.3 ~ Smatier range, smaller discretization (observed — modeled).
Figure 5.4 — Smaller range, smaller discretization (observed*4.8 — modeled) .

5.3.2 HEDR Codes Correction FactOr.......0+.0»
Figure 5.5 ~ Corrected 1951 data (observed"4.8 — modeled
Figure 5.6 — Corrected 1951 data: observed and-correction factor applied to modeled
values ....

6.0 Conclusions

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AAKlemsntiey Estimation of the Pu-239 Releases to the. ‘Atmosphere from the Hanford Site. December 21, 1995.
Report to Tom Hi, Foulds, Hanford Litigation Office, Seattle,

10. FINDINGS

Estimates of Pu-239 releases pertaining to different periods of time were compared in this
Teport with corresponding figures reported in the HEDR. publication [He94]. Four groups
of the Pu-239 emitters were analyzed in this report:

~ Separations plants stacks;

~ 100 areas reactor stacks;

- 224 concentration building roof fans;

- Z plant stack.

It was found that Pu-239 releases from 100 areas reactor stacks can be considered as
negligible when compared with the releases from the separations plant stacks.

¢ Amounts of Pu-239 released from 224 concentration building roof fans and from Z-plant
stack were comparable, or even much higher than the amounts released from the
separations plant stacks. It means that it can be expected as much as from 2Ci to 20Ci of
Pu-239 activity, in addition to the HEDR estimate. It is not clear why 224 facility and Z
Plant were excluded from the HEDR plutonium study.

¢ Total amount of Pu-239 released into the atmosphere from the separations plant stacks
in period 1944 - 1969 is estimated in HEDR as 1.75Ci. If timing of the
decontamination equipment installation is taken into account the total estimate of Pu-
239 release becomes equal to 7.7Ci. If both the alternative measurements of the
releases and the timing of the decontamination equipment installation are taken into
account, the total estimate of the Pu-239 releases becomes equal to 26.4 Ci. If (as it
was suggested in [B193] ) the PUREX release factor is considered two orders of
magnitude higher than it was suggested in HEDR, another 2Ci should be added to the
. Previous estimate making total.28.4 Ci... - - . cs

« Depending on what set of suggestions is considered, the total amount of Pu-239
released into the atmosphere in the period from December 1944 to December 1969 is
estimated in this report approximately from 10Ci to 50Ci which is significantly higher
than 1.75Ci offered in HEDR. :

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REFERENCES

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BI93

BI94

HEDR92

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MC62

$093

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Ballinger M.Y., Hall RB. 1989. A history of major Hanford operations
involving radioactive materials. PNL-6964 HEDR, Battelle, PNL, Richland,
Washington.

Blasewitz A.G. December 2, 1993. Comments RE: Radionuclide releases
to the atmosphere from Hanford operations, 1944 - 1972. Letter to
W.A.Glass.

Blasewitz A.G. September 22, 1994. Source term task responses
(September 9, 1994) to EPRP outstanding issues cited in June 17, 1994 FAY.
Carter to Shipler. Letter to M.W.Carter.

HEDR, 1992. Status of technical work. Technical Steering Panel Meeting.
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Heeb C.M. 1994. Radionuclide releases to the atmosphere from Hanford
operations, 1944 - 1972. PNWD-2222 HEDR, Battelle, PNL, Richland,
Washington.

Jacobs M.C. Anderson J.D., 1972 Radioactivity in gaseous waste
discharged from the separations facilities during 1971. ARH-2353 Ptl.,
Atlantic Richfield Hanford Company Richland, Washington.

Keene AR. 1952. Separations section. Radiation monitoring monthly

. report. September, 1952. HW-25817; General Electric Company, Hanford

Works, Richland, Washington.

McConaon D. The status of gaseous effluent monitoring at HAPO,
December 1961. 1962 HW-69205, General Electric Company. Richland,

Washington.

Soldat JK. 1993. Plutonium and Uranium releases from Hanford
separations facilities / Raw data. Memorandum to HEDR Project Office,
HEDR Project Document No. 10930320,

Uebelacker D.L. 1970, Radioactivity in gaseous waste discharged from the
separations facilities during 1969. ARH-1604., Atlantic Richfield Hanford

Company. Richland, Washington.

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AAKlemstiey Estanation ofthe Pu-239 Releases to the Atmosphere from the Hanford Site. Decewber 21, 1995.
Report to Tom H. Foulds, Hanford Litigation Office, Seattle,

Generic release ratios were calculated in [He94] by dividing the curies (Pu) of Pa-239
released during a given time period by the curies (Pu) of Pu-239 processed during that
period.

For the data presented in the Table 1, the average value Pu of the daily Pu 239 release is
0.8768 :Ci/day, found according to the formula

O Ph=am dry,
where Nis the number of measurements. In the case of Table 1 it is equal to 9.

Amount of Pu-239 processed in PUREX during December 1957 is equal to 13,500 Ci. Itis
calculated according to the formula [He94]: .

6) Pu = T*0.08382*BU - 3.331E-5*BU**2 + 9,163E-9*BU*#3 -1,16E-12*BU**4 +
+ 9.906E-5*PD*BU

where T (tons) is the mass of spent fuel processed during the month, having average burnup
BU (MW4d/ton) and power density PD (MWAtn).

Overall release factor attributed to PUREX, December 1957, is found according to
(©) ORF(12/57) = (0.8768yCi/day *31day) / 13,500 Ci=2E-9,

Release factors for the rest of the separations plants were found in the similar way. The
HEDR reconstructed values of the release factor are tepresented in Table 2.

_ Table 2

HEDR reconstructed values of the release factor

12/44-5/48 | After 5/48 | Entire period
of operation

Tand B Plant 4E-5 4E-7
REDOX 2E-7
PUREX 2E-9

The values of release factor for T and B plants related to the period 12/44-5/48 are found
under the suggestion that the overall plant efficiency for radioactive particles was 99%,

.HEDR estimates of amounts of Pu-239 released in month £ were calculated with the use of
formula

Pukey = ORF R)* PP,



AAKlementiey Estimation of the Pu-239 Releases to the Atmosphere from the Hanford Site, ‘December 21, 1995,
Repoct to Tom H. Foulds, Hanford Litigation Offica, Seattle,

where P.P() are calculated according to (2), and RF) found from Table 2.

3. BLASEWITZ” CRITICISM

Blasewitz questioned the HEDR estimation of the radionuclide releases to the atmosphere
in [B193] and [B194] where he pointed out the following three major problems:

1. Incorrect estimation of the overall release factors for the period 1944 - 1951
"The release factors, and of course, the releases [estimated in HEDR, AK from B and T
Plants for the period of 1944 until early 1951 are in error"{BI93, p.1).

2. The input data are significantly uncertain
"The data upon which the release factors ... are based are exceedingly sketchy and tenuous”
[BI93, p.1};

3. PUREX overall release factor was dramatically underestimated

“In view of the mechanisms involved in the formation of the radioactive aerosols and the
decontamination equipment used, it would be expected that the release factors for all of the
particulate radionuclides would be essentially the same fro a given separations plant and
they would be similar for all of the plants.... The release factor for plutonium at PUREX
is, however, reported [in HEDR, A.K.] as 2 orders of magnitude lower than the other
radionuclides." [B193, p.2]. :

All three aspects of Blasewitz criticism of the HEDR estimation of Pu-239 releases from
the Hanford Site were taken into consideration in the study presented in this report.

4. CHRONOLOGY

. A diagram of the B and T Plant ventilation systems and the particulate
decontamination equipment which was installed at various times and their respective
removal efficiencies compiled from [B193] is presented in Appendix B. Four major
stages in development of the emission control equipment indicated in the diagram are
depicted on Table 3.

One can see from the diagram that two different ventilation lines existed in the
processing plants: one was canyon ventilation air line, having decontamination factor
DF , and another one was dissolver off-gases line, having decontamination factor DF’.
According to [Bi93], 3,900 units of activity were vented into the off-gas line per each
10,000 units vented into the canyon ventilation system. Or, the proportion was 28% to
72%. Values of DF“) and DF) pertaining to each particular period of the emission

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AAKlementicy Estimation ofthe Pu-239 Releases to the Atmosphere from the Hanford Site, December 2}, 1995.
‘Report to Tom H. Foulds, Hanford Litigation Office, Seattle,

Table 9
Calculating release factor for Z Plant

Bates | Document | Period | Period | Adjusted [ Pu239 | Pu-239 Z Plant Averaged
mumber | number | begin end | amount | Processed | Processed} release {release factor!
Cifday jin REDOX|in PUREX| factor Q@F-Z)

2166110 | HW-59849 | 3/1/59} 3/31/59] 1.100E-05} 1930} 20700] 1.458E-63}
2159955 | HW-60915 | 6/1/59} 6/30/59] 1.671E-05} 3210] —_26300| 1.699B08|
2166134 | HW-61366 { 7/1/59} 7/31/59{ 1.130E-05| 3750} 13600] 1.9548-08}
2166155 | HW-62179 | 9/1/59} 9730/59| 2.200E-05} 2580} 19200] _3.03E-08|
2166078 | HW-62593 | 10/1/59} 10/31/59} 1.300E-05| 2790} 18600} 1.823E-03}
2159995 | HW-62864 | 11/1/59} 11/30/59] 1.620B-05| 4180] 19000} 2.097E-68]
2166214 | HW-63706 | 12/1/59} 12/31/59] 7.120E-05| 5360} 23800} 7.325E-08|

2166214 | HW-63706 | 1/1/60} 1/31/60] 1.070E-05] 837] 28800} 1.083E-03}
2160063 | HW-66646 | 8/1/60} 8/31/60] 1.0608-04| 1810} 33900} 8.905E-08|
2160076 | HW-66958 | _9/1/60{ 9/30/60] 3.6008-05} Tis 33500{ 3.151808}

2160099 | HW-67252 | 10/1/60} 10/31/60| 1.240E-05| 2960] 17900} 1.783E-08|
2160112 | HW-67459 | 11/1/60} 11/30/60] 1.271E-04] 3830 32200| 1.058E-07} 3.741E-08

150160 | HW-69205 | 12/1/6i{ 12/31/61[2.300E-05 ) 4620} 1.494E-07}
150161 | HW-69205 | 12/1/61] 12/31/61] 2.200E-05| 0} 5270|_1.252E-07}
150161 | HW-69205 | 12/1/61] 12/31/61 1.500E-05| 14 4980} 9.011E-08)
150161 | HW-69205 | 12/1/61} 12/31/61} 1.500E-05| 5) 1560} 2,884B-07|
150161 | HW-69205 | 12/1/61] 12/31/61] 1.100B-05} Oy 3340| 9.88B-08|
150161 | HW-69205 | 12/1/61] 12/31/61] 1.700E-05| 0} 4990} 1.022E-07
150161 | HW-69205 | 12/1/61} 12/31/61] 2.000E-05| 7 2440} 2.444807]
150161 | HW-69205 | _12/1/6i| 12/31/61] 3.100E-05| 4 5530} 1.665E-07|
150161 | HW-69205 | 12/1/61] 12/31/61} 2.900E-05| 59) 3390} 2.522E-07|
150161 _{ HW-69205 | 12/161] 12/31/61{2.600E-05| 104| 3960} 1.919E-07|
p 35086t [-HW-69205 |\~12/1/61|" 12/31/61] 1.700E-05t *° 390) 2010} 2.125E-07F
150161 | HW-69205 | 12/1/61] 12/31/61] 1.000E-05| 47) 79.9] 3.546E-06} 4.557E-07

The estimated values of RF-Z are related to the period 1959 - 1961 when most of Pu-249
went to Z Plant from PUREX. Averaged value of RF-Z is 3.7E-8 for 1959 - 1960, and it is
4.6E-7 for 1961. Both estimates are significantly higher than the estimate of PUREX
release factor offered in [He94].

ll



|

AAKlementiey Estimation ‘Of the Pu-239 Releases to the Atmosphere from the Hanford Site. December 21, 1995.
‘Report to Tom H. Foulds, Hanford Litigation Office, Seattle,

7. 100 AREAS REACTOR STACKS

Measurements of the Pu-239 releases from four 100 areas reactor stacks compiled from the
source spreadsheet are presented in Table 7. The average total release of Pu-239 equal to

Table 7

Measurements of the Pu-239 releases from 100 areas reactor stacks

Bates | Reference | Stack location | Period | Period Pa-239 Averaged
No. begin end jrelease Ci/day} Pu-239
. telease
Ci/mo

17739} HW-27641}_105-F STACK] 10/8/52] 12/31/52] _1.100B-06

17740} HW-27641|_105-D STACK] _10/1/52/12/31/52| __3.100E-07]

17741} HW-27641| 105-DR STACK| 10/1/52] 12/31/52] _3.700E-071

17742) HW-27641]_103-HSTACK|  10/1/52/12/31/52|__1.100E-06| 2. 16-5

2.16E-5 Ci/month is about two orders of magnitude lower than the total release from the
processing plants stacks, So, the releases from the reactor stacks can be considered as
negligible and they are not included in the further analysis.

8. 224 CONCENTRATION BUILDING ROOF FANS

224 concentration building was located behind each canyon building. “Ventilation was
supplied to each cell (of the 224 concentration building, A.K.) by fans in the pipe gallery
and was exhausted through roof fans on’éacli cell” [Ba89, .4.13]. This statement as well
as identification of the 224 roof fans as the individual separate sources of the Pu-239
teleases (Table A1), allows one to suggest that Pu-239 exhausted from the cells was not
vented to the 200 area stack exhaust system, but it was rather vented directly to the
atmosphere.

If the last suggestion is true, ihe amounts of Pu-239 released from the 224
concentration building might be comparable, or even much higher than the amounts
released from the separations plant stacks considered in HEDR. The calculations presented
in Table 8 show that in 1952 and 1953 the releases from the 224 concentration buildings
were either comparable with the releases from the corresponding separations plant stacks,
or about one order of magnitude higher.

For example, 650 Ci was processed in T-Plant in May 1952. From this amount, 0.26
millicurie was released from the T-Plant stack during the separation process. On the next

9



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AAKiementiev Estimation of the Pu-239 Releases to the Atmosphere from the Hanford Site. December 21, 1995.
Report to Tom H. Foulds, Hanford Litigation Office, Seattle.

will enter the particulate decontamination system. As much Pu-239 activity as PU;
will be released from the decontamination system through the stack into the
atmosphere. Following notations based on this concept will be used throughont the
text:

Generic release ratio (GRR) is determined by chemical properties of the solution and
separations technology. It is defined as the portion of Pu-239 that left the solution:

(— GRR=PU7/PU;.
Decontamination factor (DF) of a filter is defined as
Q) DF = 1 - PU31PU2.

Overall release factor (ORF) is as portion of processed Pu-239 that was released
through the stack, defined as:

6) ORF = PU3/ PU; = GRR (1 - DF).

2. METHOD OF THE Pu-239 RELEASES ESTIMATION: HEDR APPROACH

HEDR estimates of Pu-239 releases were based on the records of Pu-239 release.
measurements from each separations plant vent stack, available from [S093]. For PUREX,
for example, those measurements are presented in the Table 1.

Table 1

Measurements of Pu-239 releases, Dec.1957,
_ ’ “PUREX Plant, compiled from [He94, p.4.28]

Release Date Pu-239 Release,
number. uCi/day
i RO
1 12/4-5/57 0.068
2 12/5-6/57 0.039

3 12/6-7/57 16

4 12/7-9/57 0.018
5 12/9-10/57 0.03
6 12/10-11/57 48

7 12/41-12/57 0.2

8 12/14-16/57 0.036
9 12/16-17/57 Li



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Exhibit 5



AAKlemeatiey Estnnation of the Pu-239 Releases to the Atmosphere from the Hanford Site. December 21, 1995.
Report to Tom H. Foulds, Hanford Litigation Office, Seattle

Table 5
Estimates of the overall release factor
Generic | Deo.1944-| Ratio | June 1948-[ Ratio |Nov.1948-| Ratio | Feb.1951+| Ratio
release | May 1948 | Atternat.:| Oct.1948 | Aternai.:| Jan.1951 | Atternat.: Alternat.
Tatio HEDR HEDR HEDR HEDR

17-10% | 1.7-10% | 425 | 13-10% | 325 fiazio®| 30 40-107 | 10
2.8-10* | 2.810% | 700 } 22-10% | 530 | 2010° | 50 67-107 | 17
p.8-10% | 5.8107 | 1450 | 46.10% | 1750 | 4210° | 105 | 1410° | 35

6. ESTIMATION OF THE RELEASES FROM THE SEPARATIONS PLANT
STACKS : .

Altemative estimation of Pu-239 released from the separations plant stacks in the period
from December 1944 to December 1969 was done with the use of formula (7). The
amounts of Pu-239 released after 1969 were found to be relatively small, so they were not
included in the study. Results of calculation are presented in Table 6.

Total amount of Pu-239 released into the atmosphere in period 1944 - 1969 is estimated in
HEDR as 1.75Ci. This estimate does not account for three factors pointed out in section 3
in this report, However, these three factors were taken into account when altemative
estimates were calculated. One can see from the Table 6 that if only the first factor (Le.
timing of the decontamination equipment installation) is taken into consideration, the total
estimate becomes equal to 7.7Ci.

The set of measurements of Pu-239 releases used by HEDR [$093] for the estimation of
release factor is.not the only one available from the historical zecords. Analysis of the -
additional data from the source spreadsheet allows one to suggest that releases could be up
to about 3.5 times higher than those reported in [S093]. It means that if both the alternative
measurements of the releases and the timing of the decontamination equipment installation
are taken into account, the total estimate of the Pu-239 releases becomes equal to 26.4 Ci.

If the PUREX release factor is considered two orders of magnitude higher than it was
suggested in HEDR, another 2Ci should be added to the previous estimate making total
28.4 Ci.



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